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Abstract Enhancing mass transport of reactive species and photons at the plasmaliquid interface is an important consideration for the scaling of atmospheric pressure plasmas studied in the laboratory to real-world applications. It is well-known that the introduction of turbulence at any interface will enhance mixing by enhancing species uptake from the gas phase to the liquid phase by surface renewal processes, entrainment, bubbles and surface area modification. The goal of this work is to isolate surface effects associated with turbulence from the multitude of turbulent transport enhanced processes by artificially introducing surface perturbations using Faraday waves. Experiments were also conducted to determine decoloration rate constants of a model contaminant (methylene blue) as a function of both discharge features and hydrodynamics (Faraday surface wavelengths). The local plasma ionization wave at the interfacial structure was modeled and compared to experiments. Interestingly, it was found in experiments that plasma in contact with the water also generated capillary waves thus modifying the surface as well. Plasma ionization waves in combination to acoustic driven Faraday waves adds to the complexity of interpreting the effects of, for example, surface area increases, due to these complex coupled phenomenon. Local plasma ionization wave structure appears to be modified (increased propagation distance) when the liquid is perturbed, leading to increased contact of the liquid water surface with reactive species. Along with interfacial surface area growth, nonlinear convective transport is also increased with perturbations, leading to the general realization that acoustic perturbations can improve transport and thus decoloration of the model contaminant dye.more » « less
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Abstract In an atmospheric DC glow discharge with liquid anode, the plasma attachment under certain conditions self-organize into coherent patterns at the anode. Optical emission spectroscopy revealed that attachment emission consists primarily of the second positive system of nitrogen N2(C-B) whose excitation energy is low and sensitive to the change of electron energy distribution. Besides the electrons, negative ions can also accumulate in the anode sheath and affect the local space charge. It has been conjectured that these negative ions play a role in pattern formation at the anode surface. In this work, the role of oxygen negative ions was explored. It was found that the establishment of anode patterns requires at least a 7 % volume fraction of oxygen in the ambient gas. Results showed that at least in this work, O2- is the dominant negative ion species and has a density ~10^13 cm^-3. While the presence of oxygen appears crucial to pattern formation, this study indicated that the mere presence of the negative ions itself was not sufficient for pattern formation, suggesting a more complex mechanism involving electronegative species must be present. In fact, it was found that even when as many as 67 % of negative ions in the plasma were detached, no obvious geometry changes were observed in the self-organized pattern.more » « less
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Plasma-based water purification involves the transport of reactive species across the gas–liquid interface. This process is limited by slow diffusion driven mass transport of reactive species across the interface. Additionally, the plasma gas–liquid contact area is typically limited, contributing to reduced dose delivery. These key factors make it difficult to scale up the treatment process to input flows of industrial interest. In this work, turbulence is explored as a means to introduce a fine grain structure, thus greatly increasing the interfacial surface area, leading to large property gradients and more efficient mass transport. Such a fine scale structure can also enhance the local electric field. The test apparatus explored in this work is the packed bed reactor that places thin water jets into contact with plasma. It is theorized that introducing turbulence, via increasing Reynolds number in such thin jets, may enhance the effective plasma dose at fixed plasma power. In this work, changes in the flow regime, from laminar to turbulent, of water jets in a packed bed water reactor (PBR) configuration are investigated experimentally. Methylene blue dye, a model contaminant, was tested in the PBR to demonstrate enhanced treatment via reduced treatment times. Plasma surface morphology around the jets noticeably changed with the flow regime, and turbulent flow demonstrated a faster hydrogen peroxide uptake, along with slower temperature, electrical conductivity, and a pH change in a batch treatment process, compared to laminar flow. The dye was destroyed significantly faster in the turbulent flow, indicating an increased effective plasma dose.more » « less
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Abstract The interactions between plasma and liquid solutions give rise to the formation of chemically reactive species useful for many applications, but the mass transport in the interfacial region is usually limited and not fully understood. In this work, we report on the observation and explanation of droplet ejection at the plasma–liquid interface of a one-atmosphere glow discharge with the liquid anode. The impact of droplets emission on plasma properties is also analyzed by spectroscopy. The process, which is an efficient mass and charge transport mechanism, apparently occurs during discharge operation and thus constitutes a feedback vehicle between the discharge and the liquid. Distinctive from the well-known Talyor cone droplets associated with liquid cathodes, the observed droplets originate from the bubbles due to electrolysis and solvated air which does not require strong electric field at liquid surface. Instead, the droplets are ejected by bubble cavity rupture at the plasma–liquid interface and their size, initial speed are strongly dependent on the gravity, inertia and capillarity. The droplets emerge near the plasma attachment and are subsequently vaporized, emitting intense UV and visible light, which originated from excited OH radicals and sodium derived from the liquid electrolyte. Spectroscopy analysis confirmed that the bursting droplets generally reduce the gas temperature while their effects on electron density depend on the composition of the liquid anode. Results also show that droplets from NaCl solution increase the plasma electron density due to the lower ionization potential of sodium. These findings reveal a new mechanism for discharge maintenance and mass transport as well as suggest a simple approach to dispersing plasma-activated liquid into the gas phase and thus enhancing plasma–liquid interaction.more » « less
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